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The Study of Catalytic Oxidation of Nitrogen MonoxideWang, Ching-Chie 31 July 2000 (has links)
The study of catalytic oxidation on the removal of NO was investigated over the Cu-catalysts . The Cu-catalysts , including Cu/TiO2 , Cu/Al2O3 and Cu/SiO2 , were prepared by impregnation method . Alougth NO2 , the product of this reaction , has higher toxicity than NO , but it might be removed completely by absorption with H2O or alkalinal solution for its high solubility .
The experiments can be divided into three parts , i.e. , the screen of test catalysts , the effect of operating factors on the conversion of NO and the kinetic model . In the first part , the activity of test catalysts , which were prepared by mixing three various sources of Cu-ions¡]i.e., Cu(NO3)2 , Cu(CH3COO)2 , and CuSO4¡^with three different types of support¡]i.e., TiO2 , Al2O3 , and SiO2¡^, and were compared in form of conversion on NO to find the best catalyst . The results show that the mixture Cu(NO3)2 / TiO2 has the good performance on the conversion of NO , and also has more wider operating in range of temperature . In order to find the optimal loading of Cu on Cu(NO3)2 / TiO2 , additional test of various dosage over the catalysts was conduct in series . It is found that 8wt.% of Cu loading on Cu(NO3)2 / TiO2 is the most economic dosage . Therefore , we select this type of Cu oxide as the best catalyst in the following work .
In the second part , the effect of NO inlet concentration , space velocity and humidity on the conversion of NO were performed . The results show that the conversion of NO decreases with the increasing of [NO]in when [NO]in is larger than 1000ppm¡Fthe conversion of NO is not changed with [NO]in when [NO]in is lower than 1000ppm . The better space velocity is 15000hr-1 , i.e.,the empty bed residence time is 0.24 second . The reaction on NO conversion would be restrained by higher humidity contenting in inlet gas stream , but the effect of inhibition on NO conversion is not significant .
Finally , the kinetics of the oxidation of NO over 8wt.% Cu(NO3)2 / TiO2 was obtained by integral method .It is found that the oxidations of NO can be described by first order reversible reaction and the observed activation energy are 15.8 kcal/mole¡]forward reaction¡^and 25.9 kcal/mole¡]backward reaction¡^, respectively . By comparing the conversion of predicted NO with the experimentals , we can find the suitable operation conditions in application of the kinetic model : the inlet concentration of NO in a range of 300-1000ppm , the empty-bed residence time ranging from 0.12-0.48 second , and the absolute humidity ranging from 4854 to 42475ppm .
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Effect of Oxygen Concentration and Promoters on the Performance of Copper Catalysts During Catalytic Reduction of Nitrogen MonoxideLiu, Kai-Chung 14 September 2001 (has links)
This study utilized Cu-catalysts to catalyze a NO reduction reaction using CH4 as a reductant. Due to CH4 being a weak reductant and is easily affected by O2 concentration, we undertook a series experiments with O2 concentration and promoters, so that we could better understand their influence. The experiment conditions were as follows : reaction temperature between 150¢J- 800¢J¡Fa catalysts weight of 0.5 g¡F total gas flow rate of 1000 ml/min¡Frelative humidity at 0.9 %¡Fan O2 concentration between 0 - 6%¡Fand CH4 concentration between 1000 - 10000 ppm.
First, we sorted out the best metal carriers and calcining temperature, from this we decide to use £^-Al2O3 as a carrier with a calcining temperature under 500¢Jto produce our catalysts. During the O2 concentration experiment, when the inflow O2 concentration was below 1% (including 0% O2), Cu-catalysts reduce NO above 550¢J.The conversion reached a rate of 95 % at a temperature of 750¢J¡Fwhen the oxygen concentration was between 3% and 6% O2, catalysts reacted within 300 - 500¢J with NO converting to NO2¡Fat a concentration between 1.5% and 2% O2, NOx underwent reduction at 750¢J,and NOx conversion raised from 0 % to above 90%. Therefore in analyzing the experiment results, it shows that NOx will reduce violently when the O2 concentration is below 0.7% and while using CH4 as a reductant. This result was also apparent in O2 concentrations between 1.5 % and 2%. In the experiments of M/O ratio (the ratio of CH4 and O2 inflow), we found M/O ratio was not a deciding factor within the reaction mechanics, furthermore the limiting factor of O2 concentration decreases under 0.7%¡Fin addition it was also found that adding large amounts of CH4 could quicken the reduction process. Lastly, a mass balance was performed, which had a result over 70 %.
In the experiments where Y¡BLa¡BSr¡BCo were added as promoters to the Cu-catalysts, we found that Cu-La/£^-Al2O3¡BCu-Sr/£^-Al2O3 and Cu-Co/£^-Al2O3 can accelerate O2 depletion. Henceforth, it is possible to deduce promoters will be a useful method in solving O2 limiting. In the comparison of metals loading methods, we found no difference in activity using separate-impregnation and co-impregnation methods, whereas in the BET and SEM co-impregnation experiments, there was a larger surface-area and dispersion.
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